Journal
NATURE CHEMISTRY
Volume 11, Issue 7, Pages 622-628Publisher
NATURE PUBLISHING GROUP
DOI: 10.1038/s41557-019-0263-4
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Funding
- King Abdullah University of Science and Technology [FCC/1/1972-19]
- National Natural Science Foundation of China [21771161]
- Thousand Talents Program for Distinguished Young Scholars
- Royal Society [F160062]
- EPSRC [EP/R029431/1] Funding Source: UKRI
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Defect engineering of metal-organic frameworks (MOFs) offers promising opportunities for tailoring their properties to specific functions and applications. However, determining the structures of defects in MOFs-either point defects or extended ones-has proved challenging owing to the difficulty of directly probing local structures in these typically fragile crystals. Here we report the real-space observation, with sub-unit-cell resolution, of structural defects in the catalytic MOF UiO-66 using a combination of low-dose transmission electron microscopy and electron crystallography. Ordered 'missing linker' and 'missing cluster' defects were found to coexist. The missing-linker defects, reconstructed three-dimensionally with high precision, were attributed to terminating formate groups. The crystallization of the MOF was found to undergo an Ostwald ripening process, during which the defects also evolve: on prolonged crystallization, only the missing-linker defects remained. These observations were rationalized through density functional theory calculations. Finally, the missing-cluster defects were shown to be more catalytically active than their missing-linker counterparts for the isomerization of glucose to fructose.
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